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Biomaterials Science · 2021 ·Vol. 9 ·期 24 ·8323-8334 · IF 6.843

An intrinsically thermogenic nanozyme for synergistic antibacterial therapy

Caixia Sun,Wenqian Wang,Xiaolian Sun,Weihua Chu,Jun Yang,Jianjun Dai,Yanmin Ju

Bacterial infections with a high mortality rate have become serious health issues for human beings. As natural enzymes play an important role in the survival and proliferation of bacteria, effective inhibition of bacterial natural enzyme activities is important for antimicrobial therapy. Herein, a novel enzymatic antibacterial strategy, of enhancing nanozyme activity but reducing bacterial natural enzyme activity, is developed based on yolk–shell Fe2C@Fe3O4-PEG thermogenic nanozymes with highly magnetothermal properties and thermal-enhanced peroxidase-like activities. When applying an alternating magnetic field, the special yolk–shell Fe2C@Fe3O4-PEG nanozymes show a better magnetothermal effect than Fe2C (yolk) and Fe3O4 (shell) due to the increased value of their magnetic energy product, and the peroxidase-like activity of the nanozymes is further improved. Meanwhile, remarkably restrained by the enhanced magnetothermal effect from the nanozymes, typical natural enzyme activities of bacteria are detected with an inhibition rate of nearly 80%. Both in vitro and in vivo experiments exhibit superior synergistic antibacterial efficacy. The antimicrobial mechanisms are explained as the reduction of natural enzyme activities and the disruption of cell walls and membranes induced by the self-magnetothermal effect of nanozymes along with the production of abundant ˙OH radicals derived from the thermal-enhanced peroxidase-like activity of nanozymes. Overall, this work focuses on an intrinsically thermogenic nanozyme, which provides a potential platform for future synergistic antibacterial application.

研究领域: 生物医学工程 · 微生物学 · 纳米医学
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JOURNAL OF POLYMER SCIENCE · 2021 ·Vol. 59 ·期 19 ·2201-2211 · IF 0

Spherical polyelectrolyte brushes as bio-platforms to integrate platinum nanozyme and glucose oxidase for colorimetric detection of glucose

Qingsong Yang,Li Li,Liang Sun,Zhishuang Ye,Yunwei Wang,Xuhong Guo

The integration of nanozyme and natural enzyme for cascade reactions has attracted great attention due to their huge potential applications in detection, biomedicine, and catalysis. Here the novel cascade bio-platforms were fabricated by using spherical poly[(2-methacryloyloxyethyl)trimethyl ammonium chloride] (PMOTA) brushes (SPB) as nanoreactors to prepare platinum nanoparticles in situ and as nanocarriers to immobilize glucose oxidase (GOX). The generated Pt nanoparticles possess high stability and peroxidase-like properties, which can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H 2 O 2 to generate blue colored oxidized TMB (oxTMB). And the absorbed GOX can specifically catalyze the oxidation of glucose into gluconic acid and H 2 O 2 , while the produced H 2 O 2 is subsequently catalyzed by the Pt nanozymes. Thus, the co-immobilized Pt nanozymes and GOX within SPB (SPB@Pt@GOX) acted as effective biosensors for colorimetric detection of glucose showing high selectivity and great feasibility. This work demonstrates a facile and general strategy to use SPB as bio-platforms to integrate nanozymes and natural enzymes for cascade reactions. Graphical

研究领域: 生物化学 · 纳米医学 · 分析化学
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-12 · IF 17.694

Boosting the performance of single-atom catalysts via external electric field polarization

Pan Yanghang,Wang Xinzhu,Zhang Weiyang,Tang Lingyu,Mu Zhangyan,Liu Cheng,Tian Bailin,Fei Muchun,Sun Yamei,Su Huanhuan,Gao Libo,Wang Peng,Duan Xiangfeng,Ma Jing,Ding Mengning

Single-atom catalysts represent a unique catalytic system with high atomic utilization and tunable reaction pathway. Despite current successes in their optimization and tailoring through structural and synthetic innovations, there is a lack of dynamic modulation approach for the single-atom catalysis. Inspired by the electrostatic interaction within specific natural enzymes, here we show the performance of model single-atom catalysts anchored on two-dimensional atomic crystals can be systematically and efficiently tuned by oriented external electric fields. Superior electrocatalytic performance have been achieved in single-atom catalysts under electrostatic modulations. Theoretical investigations suggest a universal “onsite electrostatic polarization” mechanism, in which electrostatic fields significantly polarize charge distributions at the single-atom sites and alter the kinetics of the rate determining steps, leading to boosted reaction performances. Such field-induced on-site polarization offers a unique strategy for simulating the catalytic processes in natural enzyme systems with quantitative, precise and dynamic external electric fields.

研究领域: 催化 · 材料科学 · 电化学 · 理论化学
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CHEMISTRY-A EUROPEAN JOURNAL · 2021 ·Vol. 28 ·期 1 ·e202102885 · IF 5.236

“Four-in-One” Nanozyme and Natural Enzyme Symbiotic System of Cu2-xSe−GOx for Cervical Cancer Therapy

Yubo Hu,Ke Wang,Cong Ye

Graphical The nanozyme@natural enzyme symbiotic system of Cu 2- x Se−GOx exhibited prominent “four-in-one” cascaded catalytic enzyme activities including catalase, peroxidase, glutathione oxidase and glucose oxidase. The ingenious Cu 2- x Se−GOx could significantly induce the accumulation of reactive oxygen species (ROS) at tumor regions; this results in a tumor microenvironment (TME)-activated “four-in-one” enzyme cascade that is lethal to cervical cancer. All in all, Cu 2- x Se−GOx can act as a high-performance and safe bioactive material for cancer treatment. Cervical cancer, as a common malignant tumor of the reproductive system, seriously threatens women‘s life and health, and is difficult to be cured by traditional treatments, such as surgery, chemotherapy and radiotherapy. Fortunately, tumor microenvironment (TME)-activated catalytic therapy with high efficiency and reduced off-target toxicity has emerged as a novel treatment model. Herein, we designed a “four-in-one” nanozyme and natural enzyme symbiotic system of Cu 2- x Se−GOx for TME-triggered cascaded catalytic enhanced cancer treatment. In response to unique TME, Cu 2- x Se with catalase activity could effectively catalyze over-expressed H 2 O 2 in cancer cells into O 2 . Subsequently, the glucose oxidase (GOx) could deplete intracellular glucose with the assistance of O 2 ; this not only achieves starvation therapy, but also regenerates H 2 O 2 to boost the generation of highly cytotoxic . OH due to the peroxidase activity of Cu 2- x Se. Moreover, although the free-radical scavenger glutathione (GSH) is overexpressed in tumor cells, Cu 2- x Se with glutathione oxidase activity could effectively consume GSH for enhanced ROS production. Thus, the “four-in-one” nanozyme@natural enzyme symbiotic system of Cu 2- x Se−GOx could induce significant ROS accumulation at the tumor regions, thus providing a potential approach for the treatment of cervical cancer.

研究领域: 癌症生物学 · 纳米技术 · 生物医学工程 · 药学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Iron-Mineralization-Induced Mesoporous Metal–Organic Frameworks Enable High-Efficiency Synergistic Catalysis of Natural/Nanomimic Enzymes

Siming Huang,Guosheng Chen,Niru Ye,Xiaoxue Kou,Rui Zhang,Jun Shen,Gangfeng Ouyang

Metal–organic frameworks (MOFs) have become a promising accommodation for enzyme immobilization and protection. However, the integration of multienzymes into MOFs may result in compromise of individual enzymatic activity. In this work, we report an iron mineralization strategy to facilely construct a mesoporous MOF, possessing excellent peroxidase-mimic bioactivity. Furthermore, the feasibility of in situ encapsulating natural enzymes within the developed mesoporous MOF nanozymes endows these natural/nanomimic enzyme hybrids with remarkably enhanced synergistic catalysis ability. Such activity enhancement is mainly due to (1) the fast flux rate of substances through the interconnected mesoporous channels and (2) the simultaneously increased loading amount of enzymes and iron within the MOFs caused by the iron mineralization process.

研究领域: 材料科学 · 生物化学 · 催化 · 纳米技术
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JOURNAL OF NANOBIOTECHNOLOGY · 2022 ·Vol. 20 ·期 1 ·1-15 · IF 9.429

Nanozyme-natural enzymes cascade catalyze cholesterol consumption and reverse cancer multidrug resistance

Du Bin,Zheng Mei,Ma Huizhen,Huang Jingshu,Jiao Qingqing,Bai Yimeng,Zhao Mengmeng,Zhou Jie

Multidrug resistance is still a major obstacle to cancer treatment. The most studies are to inhibit the activity of the drug transporter P-glycoprotein (P-gp), but the effect is not ideal. Herein, a nanosystem was built based on cascade catalytic consumption of cholesterol. Cholesterol oxidase (natural enzyme, COD) was immobilized on the carrier (NH2-MIL-88B, MOF) through amide reaction, COD catalyzed the consumption of cholesterol, the reaction product H2O2 was further produced by the MOF with its peroxidase-like activity to produce hydroxyl radicals (•OH) with killing effect. Due to the high expression of CD44 receptor on the surface of tumor cells, we encapsulated chondroitin sulfate gel shell (CS-shell) with CD44 targeting and apoptosis promoting effect on the surface of DOX@MOF-COD nanoparticles, which can accurately and efficiently deliver the drugs to the tumor site and improve the effect of reversing drug resistance. Taking drug-resistant cell membrane as "breakthrough", this paper will provide a new idea for reversing multidrug resistance of tumor.Graphical Abstract

研究领域: 纳米技术 · 癌症生物学 · 药物科学 · 酶学 · 药物递送系统
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 2 ·1-12 · IF 5.3

Modular coupling MOF nanozyme with natural enzyme on hollow fiber membrane for rapid and reusable detection of H2O2 and glucose

Ma Shuyan,Wei Chenjie,Bao Yuheng,Liu Yanhui,Jiang Hong,Tong Weijun,Chen Dajing,Huang Xiaojun

A novel strategy based on gradient porous hollow fiber membrane (GPF) is proposed for the modular assembly of enzyme-nanozyme cascade systems. The porous structure of GPF provided sufficient specific surface area, while the gradient structure effectively minimized the leaching of enzymes and nanozymes. To enhance stability, we prepared and immobilized metal–organic framework (MOF) nanozymes, resulting in the fabrication of GPF-MOF with excellent stability and reusability for colorimetric H 2 O 2 detection. To improve specificity and expand the detection range, micro-crosslinked natural enzymes were modularly assembled, using glucose oxidase as the model enzyme. The assembled system, GPF-mGOx@MOF, achieved a low detection limit of 0.009 mM and a linear range of 0.2 to 11 mM. The sensor retained 87.2% and 80.7% of initial activity after being stored for 49 days and 9 recycles, respectively. Additionally, the reliability of the biosensor was validated through glucose determination of human blood and urine samples, yielding comparable results to a commercial glucose meter. Graphical Abstract

CAS / MDL: 9001-37-0
研究领域: 生物传感器 · 纳米技术 · 分析化学 · 生物医学工程
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Catalysis Science & Technology · 2024 · IF 4.4

New synthetic strategy toward a natural enzyme–nanozyme hybrid dual-function nanomotor and its application in environmental remediation

Shuo Gao,Chenzhang Liu,Xiaohan Yang,Ziwei Lan,Min Zuo,Ping Yang,Jia Li

Self-driven micro–nanomotors hold great promise for environmental monitoring and remediation. However, developing a nanomotor with dual functions of colorimetric detection and degradation is still a considerable challenge. In this paper, a novel nanomotor with both selective and catalytic activities was synthesized using a combination of natural enzymes and nanozymes. The nanomotor was modeled on natural mineral halloysite nanotubes (HNTs) and had a unique layered structure. MnO2 in the inner layer was the fuel catalytic unit, which achieved actuation by catalyzing hydrogen peroxide (H2O2) to produce oxygen bubbles, and the diffusion coefficient of the nanomotor could reach 2.65 μm2 s−1 in 5% H2O2 solution. Lac/Fe-BTC@NiFe-LDH in the outer layer was the catalytic functional unit, where Lac/Fe-BTC@NiFe-LDH not only exhibited high peroxide-like active enzyme activity, but also provided abundant active sites for the loading of natural laccase. The integration of natural enzymes and nanozymes provided the material with stronger catalytic activity, which could detect the target pollutant minocycline (MC) in water more sensitively and degrade it efficiently, and provided a new idea for the removal of antibiotics from water.

研究领域: 环境科学 · 纳米技术 · 催化 · 材料科学
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Nanoscale Advances · 2023 · IF 4.7

Rapid and sensitive detection of alkaline phosphatase and glucose oxidase activity through fluorescence and colorimetric dual-mode analysis based on CuO NPs@ZIF-8 mediated enzyme-cascade reactions

Guo-Ying Chen,Mao-Ling Luo,Li Chen,Tong-Qing Chai,Jia-Li Wang,Ling-Xiao Chen,Feng-Qing Yang

The combined application of nanozymes and natural enzymes has received widespread attention in recent years. In this work, a simple and efficient method was used to synthesize a composite material of CuO nanoparticles modified zeolitic imidazolate framework-8 (CuO NPs@ZIF-8) with multiple enzyme activities (glucose oxidase-like and hydrolase-like activities) to detect the activity of natural enzymes through fluorescence and colorimetric (UV-Vis) dual-mode detections. The hydrolase- and oxidase-like activities of CuO NPs@ZIF-8 show an acceptable affinity with L-ascorbic acid 2-phosphate trisodium (AAP) and o-phenylenediamine (OPD). Using the developed sensor, highly sensitive detection of natural enzymes glucose oxidase (GOX) and alkaline phosphatase (ALP) was achieved through both fluorescent and colorimetric analysis with a wide linear range (fluorescence for GOX: 0.86-1.23×105 mU/mL, UV-Vis for GOX: 0.081-1.62×105 mU/mL; fluorescence for ALP: 0.042-1.20×104 mU/mL, UV-Vis for ALP: 0.0046-1.23×104 mU/mL) and low LOQs (fluorescence for GOX: 0.86 mU/mL, UV-Vis for GOX: 0.081 mU/mL; fluorescence for ALP: 0.042 mU/mL, UV-Vis for ALP: 0.0046 mU/mL). Compared to the other fluorescent and colorimetric sensors, this sensor has better catalytic activity due to the addition of GOX and ALP, which can amplify the detection signal and improve the sensitivity. This is the first time that composite material CuO NPs@ZIF-8 with "tandem enzyme" activity was synthesized and applied in the detection of enzyme activity. Additionally, the proposed fluorescent and UV-Vis platforms exhibit the capability to detect GOX and ALP in serum samples with satisfactory recovery, indicating potential application prospects in biochemical analysis.

研究领域: 分析化学 · 生物化学 · 纳米技术 · 材料科学
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ANALYTICAL SCIENCES · 2024 · IF 1.8

Fabrication of natural enzyme-covered / amino-modified Pd-Pt bimetallic-doped zeolitic imidazolate framework for ultrasensitive detection of metabolites

Bai Chen-Chen,Lang Jin-ye,Wang Xin-yu,Zhao Jia-meng,Dong Lin-Yi,Liu Jun-Jie,Wang Xian-Hua

Abstract The present article introduced an natural enzyme-covered/amino-modified Pd–Pt bimetallic-doped zeolitic imidazolate framework (NAPPZ) for ultrasensitive and specific detection of glucose. The dodecahedral nanomaterial zeolitic imidazolate framework (ZIF-8)-loaded Pd–Pt bimetallic nanoparticles endowed the composite with peroxidase-like activity. The modification with glucose oxidase (GOx) facilitated the rapid access of H 2 O 2 produced through glucose oxidation to the Pd–Pt nanoparticles vicinity reducing diffusion. GOx specifically catalyzes the transformation of glucose into H 2 O 2 , which then H 2 O 2 rapidly migrates to the Pd–Pt nanoparticles, catalyzing the oxidation of colorless o-phenylenediamine into the orange–yellow product 2,3-diaminophenazine. Based on the aforementioned cascade reaction, the NAPPZ and NAPPZ based on ChOx were utilized for detecting glucose in human urine samples and cholesterol in milk, respectively. The NAPPZ strategy presented a broad detection range (20–1100 μmol L −1 ) and a low detection limit (15.9 μmol L −1 ) for glucose, and the NAPPZ based on ChOx strategy approach offered a broad detection range (10–500 μmol L −1 ) and low detection limit (6.4 μmol L −1 ) for cholesterol. Therefore, this novel method holds significant potential in the areas of clinical diagnostics and food safety. Graphical abstract

CAS / MDL: 127-09-3
研究领域: 材料科学 · 分析化学 · 生物技术 · 临床诊断 · 食品安全
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